Catalytic CO reduction using photogenerated hydrides: Tuning the "hydricity"

Patrick D. Achord, James T. Muckerman, Etsuko Fujita

Research output: Chapter in Book/Report/Conference proceedingConference contribution


Producing methanol from CO2 would make valuable fuel from potentially dangerous waste. Nature shows the way in its photosynthetic use of the hydride-donor NADPH. That molecule was the inspiration for Tanaka's pbn (pbn = 2-(2-pyridyl-benzo[b]-1.5-napthyridine), the doubly reduced/doubly protonated pbnHH form of which presumably electrocatalytically reduced acetone to isopropanol (Angew. Chem. Int. Ed. 2005, 44, 5891-5894). Fujita et al. prepared Ru(pbnHH)(bpy)22+ (bpy = 2,2'-bipyridine) by irradiating Ru(pbn)(bpy)22+ with visible light (Angew. Chem. Int. Ed. 2007, 46, 4169-4172). The mechanism involves pooling two photons in a disproportionation step (Fujita et al., Inorg. Chem. 2008, in press). Our DFT calculations indicate that it may be possible to harvest a third photon to form the triply reduced, doubly protonated Ru(pbnHH.-)(bpy)2+. Our calculations also indicate that this molecule is sufficiently "hydritic" to reduce a metal-bound carbonyl on CpReNO(CO)2. Spin density calculations are consistent with the proposed mechanism.

Original languageEnglish
Title of host publicationAmerican Chemical Society - 236th National Meeting and Exposition, Abstracts of Scientific Papers
Publication statusPublished - Dec 1 2008
Event236th National Meeting and Exposition of the American Chemical Society, ACS 2008 - Philadelpia, PA, United States
Duration: Aug 17 2008Aug 21 2008

Publication series

NameACS National Meeting Book of Abstracts
ISSN (Print)0065-7727


Other236th National Meeting and Exposition of the American Chemical Society, ACS 2008
CountryUnited States
CityPhiladelpia, PA

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)

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